Understanding and controlling the carbon/electrolyte interface is key to the development of next-generation carbon-based supercapacitors for energy storage. However, many mechanistic details remain enigmatic, including the complex interplay between the electric double layer (EDL) response and electrode quantum capacitance, and how the EDL is governed by the intrinsic morphology and electronic structure of the electrode. In this work, we employed a mixed quantum-classical approach that combines the reference interaction site model (RISM) with planewave-based density functional theory to investigate the capacitive performance of the hybrid C<sub>60</sub>/graphene electrode in common aqueous electrolytes. We find that the unique curvature effects and charge localization of the hybrid system play a key role in improving the EDL response, which ultimately dominates the overall enhancement in the capacitive performance compared to pristine graphene. Our study highlights the strong interdependence of electrode electronic structure and morphology in determining the device capacitance as well as the important role played by the electrolyte. We also further discuss potential strategies for optimizing fullerene-based electrode materials with enhanced performance and stability by integrating our theoretical findings with direct electrochemical measurements.

Unravelling the enhanced capacitive performance of hybrid C<sub>60</sub>/graphene electrodes with first-principles simulations

2019 Fall National Meeting

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Unravelling the enhanced capacitive performance of hybrid C60/graphene electrodes with first-principles simulations

Unravelling the enhanced capacitive performance of hybrid C₆₀/graphene electrodes with first-principles simulations